Ce(IV)/Ce(III) redox cycle triggers hydroxyl radical production on the CeOx/carbon black flow-anode for electro-oxidation of acetaminophen

被引:1
|
作者
Jin, Huachang [1 ,4 ]
Xu, Xiaozhi [1 ]
Liu, Renlan [1 ]
Wu, Xiaobo [5 ]
Chen, Xueming [3 ]
Zheng, Xiangyong [1 ]
Zhao, Min [1 ]
Yu, Yang [2 ]
机构
[1] Wenzhou Univ, Coll Life & Environm Sci, Natl & Local Joint Engn Res Ctr Ecol Treatment Tec, Wenzhou 325035, Zhejiang, Peoples R China
[2] Zhejiang Ocean Univ, Natl & Local Joint Engn Res Ctr Harbor Oil & Gas S, Zhejiang Key Lab Petrochem Environm Pollut Control, Zhoushan 316022, Zhejiang, Peoples R China
[3] Zhejiang Univ, Coll Environm & Resources Sci, 866 Yuhangtang Rd, Hangzhou 310058, Peoples R China
[4] Wenzhou Univ, Inst Ecoenvironm Res Sanyang Wetland, Wenzhou 325035, Zhejiang, Peoples R China
[5] Ecol Environm Protect Adm Law Enforcement Team Rui, Wenzhou 325035, Zhejiang, Peoples R China
基金
中国国家自然科学基金;
关键词
Electro-oxidation; Acetaminophen; Ce(IV)/Ce(III) redox cycle; Hydroxyl radicals; CeO x /CB flow-anode; ENHANCED ELECTROCATALYTIC REMOVAL; DYEING WASTE-WATER; ELECTROCHEMICAL DEGRADATION; ELECTRODES; OXIDATION; KINETICS; PARTICLES;
D O I
10.1016/j.cej.2024.149195
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Electrochemically active materials can effectively alleviate mass transfer restriction by adding them as flowanodes into the electrochemical reactor. However, conventional flow-anode materials display a low center dot OH yield. Here, a novel flow-anode, CeOx/carbon black (CB), demonstrates superior electrocatalytic degradation efficiency of organic pollutants. The acetaminophen degradation kinetic constant of CeOx/CB was calculated to be 2.3-2.9 times higher than that of CB. CeOx/CB achieved a higher current efficiency of 66.4 % and relatively lower energy consumption of 157.8 kWh/kg COD compared with other GAC or gamma-Al2O3-based flow-anodes. The mechanistic analyses demonstrated that rapid electron transfer, strong water adsorption, and low reaction energy barrier of CeOx/CB actuated efficient center dot OH generation. Moreover, Ce(IV)/Ce(III) redox cycle crucially acted as an "electron porter" to accelerate the electron transfer from adsorbed H2O molecules to CB substrate directionally in the electro-oxidation process. This work provides a feasible manner for the development of flow-anodes utilizing the advantage of the Ce(IV)/Ce(III) redox cycle.
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页数:10
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